skip to main content

DOE PAGESDOE PAGES

Title: Dynamic layer rearrangement during growth of layered oxide films by molecular beam epitaxy

The A n+1B nO 3n+1 Ruddlesden–Popper homologous series offers a wide variety of functionalities including dielectric, ferroelectric, magnetic and catalytic properties. Unfortunately, the synthesis of such layered oxides has been a major challenge owing to the occurrence of growth defects that result in poor materials behaviour in the higher-order members. To understand the fundamental physics of layered oxide growth, we have developed an oxide molecular beam epitaxy system with in situ synchrotron X-ray scattering capability. We present results demonstrating that layered oxide films can dynamically rearrange during growth, leading to structures that are highly unexpected on the basis of the intended layer sequencing. Theoretical calculations indicate that rearrangement can occur in many layered oxide systems and suggest a general approach that may be essential for the construction of metastable Ruddlesden–Popper phases. Lastly, we demonstrate the utility of the new-found growth strategy by performing the first atomically controlled synthesis of single-crystalline La 3Ni 2O 7.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [4] ;  [2] ;  [4] ;  [6] ;  [4] ;  [4] ;  [4] ;  [2] ;  [4] ;  [4]
  1. Argonne National Lab. (ANL), Argonne, IL (United States); Korea Atomic Energy Research Institute, Daejeon (Republic of Korea)
  2. Univ. of Wisconsin, Madison, WI (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
  5. Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Science and Technology of China, Anhui (China)
  6. Univ. of Connecticut, Storrs, CT (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 13; Journal Issue: 9; Journal ID: ISSN 1476-1122
Publisher:
Nature Publishing Group
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Materials Sciences and Engineering Division; University of Wisconsin-Madison, Materials Research Science and Engineering Center (MRSEC)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; design; synthesis and processing; surfaces; interfaces and thin films
OSTI Identifier:
1357212

Lee, J. H., Luo, G., Tung, I. C., Chang, S. H., Luo, Z., Malshe, M., Gadre, M., Bhattacharya, A., Nakhmanson, S. M., Eastman, J. A., Hong, H., Jellinek, J., Morgan, D., Fong, D. D., and Freeland, J. W.. Dynamic layer rearrangement during growth of layered oxide films by molecular beam epitaxy. United States: N. p., Web. doi:10.1038/NMAT4039.
Lee, J. H., Luo, G., Tung, I. C., Chang, S. H., Luo, Z., Malshe, M., Gadre, M., Bhattacharya, A., Nakhmanson, S. M., Eastman, J. A., Hong, H., Jellinek, J., Morgan, D., Fong, D. D., & Freeland, J. W.. Dynamic layer rearrangement during growth of layered oxide films by molecular beam epitaxy. United States. doi:10.1038/NMAT4039.
Lee, J. H., Luo, G., Tung, I. C., Chang, S. H., Luo, Z., Malshe, M., Gadre, M., Bhattacharya, A., Nakhmanson, S. M., Eastman, J. A., Hong, H., Jellinek, J., Morgan, D., Fong, D. D., and Freeland, J. W.. 2014. "Dynamic layer rearrangement during growth of layered oxide films by molecular beam epitaxy". United States. doi:10.1038/NMAT4039. https://www.osti.gov/servlets/purl/1357212.
@article{osti_1357212,
title = {Dynamic layer rearrangement during growth of layered oxide films by molecular beam epitaxy},
author = {Lee, J. H. and Luo, G. and Tung, I. C. and Chang, S. H. and Luo, Z. and Malshe, M. and Gadre, M. and Bhattacharya, A. and Nakhmanson, S. M. and Eastman, J. A. and Hong, H. and Jellinek, J. and Morgan, D. and Fong, D. D. and Freeland, J. W.},
abstractNote = {The An+1BnO3n+1 Ruddlesden–Popper homologous series offers a wide variety of functionalities including dielectric, ferroelectric, magnetic and catalytic properties. Unfortunately, the synthesis of such layered oxides has been a major challenge owing to the occurrence of growth defects that result in poor materials behaviour in the higher-order members. To understand the fundamental physics of layered oxide growth, we have developed an oxide molecular beam epitaxy system with in situ synchrotron X-ray scattering capability. We present results demonstrating that layered oxide films can dynamically rearrange during growth, leading to structures that are highly unexpected on the basis of the intended layer sequencing. Theoretical calculations indicate that rearrangement can occur in many layered oxide systems and suggest a general approach that may be essential for the construction of metastable Ruddlesden–Popper phases. Lastly, we demonstrate the utility of the new-found growth strategy by performing the first atomically controlled synthesis of single-crystalline La3Ni2O7.},
doi = {10.1038/NMAT4039},
journal = {Nature Materials},
number = 9,
volume = 13,
place = {United States},
year = {2014},
month = {8}
}